Institut des Matériaux and Institut des Sciences et Ingénierie Chimiques, Laboratoire des Polymères, École Polytechnique Fédérale de Lausanne (EPFL) , Bâtiment MXD, Station 12, CH-1015 Lausanne, Switzerland.
ACS Appl Mater Interfaces. 2015 Mar 4;7(8):4631-40. doi: 10.1021/am507927w. Epub 2015 Feb 20.
Tight regulation of blood glucose levels of diabetic patients requires durable and robust continuous glucose sensing schemes. This manuscript reports the fabrication of ultrathin, phenylboronic acid (PBA) functionalized polymer brushes that swell upon glucose binding and which were integrated as the sensing interface in a new polypropylene hollow fiber (PPHF)-based hydraulic flow glucose sensor prototype. The polymer brushes were prepared via surface-initiated atom transfer radical polymerization of sodium methacrylate followed by postpolymerization modification with 3-aminophenyl boronic acid. In a first series of experiments, the glucose-response of PBA-functionalized poly(methacrylic acid) (PMAA) brushes grafted from planar silicon surfaces was investigated by quartz crystal microbalance with dissipation (QCM-D) and atomic force microscopy (AFM) experiments. The QCM-D experiments revealed a more or less linear change of the frequency shift for glucose concentrations up to ∼10 mM and demonstrated that glucose binding was completely reversible for up to seven switching cycles. The AFM experiments indicated that glucose binding was accompanied by an increase in the film thickness of the PBA functionalized PMAA brushes. The PBA functionalized PMAA brushes were subsequently grafted from the surface of PPHF membranes. The hydraulic permeability of these porous fibers depends on the thickness and swelling of the PMAA brush coating. PBA functionalized brush-coated PPHFs showed a decrease in flux upon exposure to glucose, which is consistent with swelling of the brush coating. Because they avoid the use of enzymes and do not rely on an electrochemical transduction scheme, these PPHF-based hydraulic flow sensors could represent an interesting alternative class of continuous glucose sensors.
糖尿病患者血糖水平的严格控制需要持久和稳健的连续血糖传感方案。本文报告了超薄膜状的苯硼酸（PBA）功能化聚合物刷的制造，这些聚合物刷在结合葡萄糖后会发生溶胀，并被整合为新型基于聚丙烯中空纤维（PPHF）的液压流量葡萄糖传感器原型中的传感界面。聚合物刷通过引发原子转移自由基聚合（SI-ATRP）制备，单体为甲基丙烯酸钠，随后通过 3-氨基苯硼酸的后聚合修饰。在一系列实验中，通过石英晶体微天平（QCM-D）和原子力显微镜（AFM）实验研究了苯硼酸功能化聚（甲基丙烯酸）（PMAA）刷在平面硅表面上的葡萄糖响应。QCM-D 实验表明，对于高达约 10mM 的葡萄糖浓度，频率偏移的变化或多或少呈线性变化，并且表明葡萄糖结合对于多达七个开关循环是完全可逆的。AFM 实验表明，葡萄糖结合伴随着 PBA 功能化 PMAA 刷的膜厚度增加。随后，PBA 功能化 PMAA 刷从 PPHF 膜表面接枝。这些多孔纤维的液压渗透率取决于 PMAA 刷涂层的厚度和溶胀。暴露于葡萄糖后，PBA 功能化刷涂的 PPHF 通量下降，这与刷涂层的溶胀一致。由于它们避免使用酶并且不依赖于电化学转换方案，这些基于 PPHF 的液压流量传感器可以成为一类有前途的连续葡萄糖传感器。
